Synergistic effects of defects and surface engineering in Ni-Co metal oxides to improve the high performance of Zn-ion hybrid supercapacitors

NiCo₂O₄ (NCO) is an auspicious pseudocapacitor material for high energy density zinc-ion hybrid supercapacitors (ZHSCs), but its low intrinsic conductivity and significant volume expansion seriously hinder its electrochemical performance. Here, we develop a nitrogen (N) doped and oxygen-vacancy-rich (Ov) Ni–Co oxide nanolines grown in-situ on the carbon cloth (CC) named N-Ov-NCO@CC. The morphology and structure of N-Ov-NCO@CC were characterized by XRD, XPS, EPR, SEM and TEM. It can be clearly observed that N-Ov-NCO@CC nanowires are composed of many tiny nanoparticles, and this unique structure provides abundant gaps at the microscopic scale, providing ample sites for the attachment of electrolyte ions. Due to N-functionalization, synergistic effects of doping, defect and surface engineering are realized. As a result, N-Ov-NCO@CC exhibits significantly enhanced electrochemical performance. The N-Ov-NCO@CC single electrode exhibits a high capacitance of 993.0 F/g (496.5C/g) at 1 A/g and excellent cycle stability with a capacitance retention rate of 98 % after 5000 cycles. In addition, the assembled N-Ov-NCO@CC//Zn-ZHSC operates stably in the voltage range of 1.2–2.0 V. A high specific capacitance of 484.4 F/g is available at current densities of 1 A/g. In addition, it still has a high cycle life with a capacitance retention rate of 97.1 % after 10,000 cycles and a high specific energy/power (50.3 Wh/kg at 300.2 W/kg). Density function theory (DFT) verification shows that N-Ov-NCO has higher conductivity than Ov-NCO and pristine NCO, which is conducive to improving electrochemical performance. This work provides a new idea for developing stable electrode materials for new ZHSCs.